Geochemical Assessment of Heavy Metal Contamination in Coastal Sediment Cores From Usukan Beach, Kota Belud, Sabah, Malaysia

Journal of Physics: Conference Series
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14th Seminar on Science and Technology 2021 (S&T 2021) IOP Publishing
Journal of Physics: Conference Series 2314 (2022) 012008 doi:10.1088/1742-6596/2314/1/012008
GEOCHEMICAL ASSESSMENT OF HEAVY METAL

CONTAMINATION IN COASTAL SEDIMENT CORES
FROM USUKAN BEACH, KOTA BELUD, SABAH,
MALAYSIA
Ling S Y1, Junaidi A1, Mohd Harun A1,2 and Baba M*1,2
1
Geology Department, Faculty of Science and Natural Resources,
Universiti Malaysia Sabah, 88400 Kota Kinabalu, Sabah, Malaysia.
2
Small Island Research Centre, Faculty of Science and Natural Resources,
Universiti Malaysia Sabah, 88400 Kota Kinabalu, Sabah, Malaysia.
*Email: babamus@ums.edu.my
Abstract. This article discussed on the status of heavy metals (As, Cr, Cu, Mn, Ni, Pb and Zn)
pollution in coastal sediment cores and assess the sediment quality from Usukan Beach, Kota
Belud. Several geochemical parameter analyses such as pH, moisture content (MC), organic
matter (OM) and granulometric size were performed to identify the physico-chemical properties
of sediments that affect the assessment of metal pollution. Heavy metals in the sediment samples
were extracted using aqua regia methods and Inductively Coupled Plasma Optical Emission
Spectrometry (ICP-OES) were employed for determination of heavy metals in extracted
sediment solutions. The results show that the coastal sediment changes from acidic to alkaline
when heading from inland to seaward direction, with an average pH of 5.6-8.5. The moisture
content and organic matter fluctuate from low to moderately high, within the range of 4.9-21.9%
and 0.30-6.73%, respectively. The coastal sediments are dominated by a sandy texture near the
marine environment and change to sandy loam and sandy clay loam when heading toward the
inland. The hierarchical average metal concentration shows Fe>Mn>Ni>Cr>Zn>Cu>Pb>As.
Sediment quality assessment is evaluated based on the sediment quality guidelines (SQGs) and
from the pollution indices such as geoaccumulation index (Igeo), enrichment factor (EF),
contamination factor (CF), modified degree of contamination (mCd) and pollution load index
(PLI). The results indicated the sediment has only low degree of contamination by anthropogenic
sources and the current status of the study area is safe from pollution.
Keywords: Geochemistry, Heavy Metal, Contamination, Sediment Quality, Coast
1. Introduction
Heavy metals are lethal, resistant, insoluble, non-biodegradable and can cause serious concern to the
environment and humans through biological or chemical processes [1,2]. The deposited heavy metals
may re-enter and remobilized from the sediments into the marine water system and bioaccumulate in
bodies of marine organisms. These marine organisms have the potential as carriers of transfer,
accumulation and settlement for heavy metals into the ecosystem or human bodies that pose risks to
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human and environmental health [3,4]. Metal contaminants in food chain when consumed might induce
food poisoning, neurological diseases or even deaths such as the Minamata disease in Japan and
Paralytic Shellfish Poisoning (PSP) in Sabah [5,6].
Coastal sediments are sensitive indicators when evaluating heavy metals that are continuously
added either from terrestrial origins such as parent materials, crustal earth, oceanographic setting and
atmospheric pollutants; or human interpolation including socioeconomic development or industrial,
agricultural and domestic waste [7,8,9]. The sediment cores are collected near the coastal environment
where the ocean basin acts as the principal reservoir for the deposition of sediment or any heavy metal
burden transported during orographic precipitation from hilly terrains [10,11]. The deposited heavy
metals that have been trapped in coastal sediments will be also be released, remobilized and resuspend
back into the marine water system due to any changes in the sediment properties or environmental
conditions. This signifies those coastal sediments not only serve as a natural reservoir for heavy metal
burden, but also as secondary source of metal pollution to the marine system [12].
Coastal sediments are also greatly influenced by the continuous erosional effect from storm-
wave actions and rebuild by the sediment transport or aeolian transport processes to the landward
direction [13,14,15]. The cohesive and adhesive forces within the wet sand grains on surface sediments
are induced by the surface moisture which hold and resist the uppermost layer of beach sediments from
being eroded into the ocean [16,17]. The resuspension of heavy metals from coastal sediments due to
sea turbulence, the movement of benthic organisms and intertidal waves or currents also determine the
pollution pattern of marine ecosystem [18,19]. Therefore, the marine environment is a complex
ecosystem, where the natural occurrence of coastal erosion, weathering and acidification processes
further facilitate the release of these metals into the marine ecosystem.
When the heavy metal concentrations from the geological background surpassed the range of
acceptable standard limits or are significantly enriched by anthropogenic sources, they may become
extremely toxic even at very low concentrations [20]. Therefore, the standard limits established in
Sediment Quality Guidelines (SQG) are used to determine whether the total metal contents are within
allowable concentration limits and to monitor the eco-toxicity level or quality of the coastal sediments
[21,22]. The present study thus serves as a baseline to monitor and evaluate the current status and extend
of metal contamination in the coastal environment of Usukan beach. The objectives of this research are
(1) to determine the heavy metal concentrations in coastal sediments, (2) to determine the possible
sources of heavy metals and (3) to assess the sediment quality of the study area.
2. Materials and Methodology
2.1. Sampling Location and Technique

Kota Belud is located at the northwest coast of Sabah, Malaysia, which is bounded by the South China
Sea and is made up of Crocker Formation from Eocene to Early Miocene, Wariu Formation from Middle
Miocene and Quaternary Alluvium [23]. The major rock units underlying Kota Belud are interbedded
sandstone, siltstone and shale units from Crocker Formation; and a mixture of chaotic rock deposits
from different origins and age including chert-spilite, limestone, breccia and ophiolitic rocks from Wariu
Formation [24,25,26,27]. The Quaternary alluvial deposits are from the weathering and pedogenesis of
the underlying parent rocks (Crocker and Wariu Formation) eroded and transported from higher terrains
to the beach shoreface and are mixed with recent coral fragments aging from Pleistocene to Quaternary
along the beach coastline. Station 1 (Samples SP2, SP3, S1A, S1B), Station 2 (Samples S2A, S2B, S2C,
S2D) and Station 3 (Samples S3A, S3B) are located in the alluvial region, whereas Station 4 (Samples
S4A, S4B, SM1, SM2) is located within the Crocker Formation, whereby this geological background
affects the geochemical distribution of heavy metals in the study area.
2
The study area is located along the coastal region at Usukan beach which lies within a latitude
of 6 17’ 40”N to 60 36’ 50”N and longitude of 1160 16’ 50”E to 1160 33’ 0”E (Figure 1). In this study,
0
a total of fifty-three (53) sediment samples were collected from four (4) sampling stations which were
carefully collected using a sediment core sampler and PVC pipes with diameter 10 cm and length 100
cm. The core samples were closed tightly using the Styrofoam cork to avoid contamination before
extruded using horizontal extrusion method to remove the sediment cores from the PVC pipes. The
samples were then sliced and divided into every 10 cm thick sub-samples and kept in airtight
polyethylene bags that were taken to the laboratory for further analysis.
Figure 1. Geological map of the study area and sampling stations in Kota Belud, Sabah.
(Source: Jabatan Mineral dan Geosains Malaysia [28])
2.2. Laboratory Analysis

The laboratory analyses conducted were pH, moisture content (MC), organic matter (OM) and
granulometric size to determine the physico-chemical characteristics of sediments based on British
Standard Method [29]. The pH analysis was conducted immediately once the fresh samples were
extruded (BS 1377-3: 1990, (Part 9.5)), whereas the samples for MC were dried at 1050C for 8 hours
using the conventional oven method (BS 1377-2: 1990 (Part 3.2)). The samples for OM were dried
overnight in a furnace at 4000C with the dry combustion method (BS 1377-3: 1990 (Part 4.3)), whereas
air-dried samples were used for granulometric size analysis with the dry sieve-pipette method (BS 1377-
2: 1990, (Part 9.3-9.4)). The samples were digested with aqua regia method to extract heavy metals.
3
Extraction method follow USEPA 3050b which use HCL:HNO3 acid with 3:1 ratio [30]. Digested
solutions were then filtered through 0.45 µm Whatman filter membrane and the filtered solution volume
were made up to 50 mL. Heavy metals in solution were detected using ICP-OES model Perkin Elmer
Optima 5300DV spectrometer.
2.3. Statistical Analysis

The contamination levels of As, Cr, Cu, Mn, Ni, Pb and Zn elements in the coastal sediment cores were
evaluated using the Igeo, EF, CF, mCd and PLI parameters to assess the sediment quality based on the
world’s average shale values [31] and by comparing the heavy metal concentrations with the SQGs by
US EPA [32] legislation as reference. A multivariate analysis was performed via the IBM SPSS
Statistics 27 software for Windows. The Pearson correlation matrix was performed to determine the
correlation and linkage between the physico-chemical parameters and total means of heavy metals at
significance levels of p<0.05 and p<0.01.
3. Results
3.1. Physico-chemical Properties

From Table 1, the geochemical parameters determined are the arithmetic mean and standard deviation
for pH (7.29±0.98), moisture content (25.3±12.94%), organic matter (1.27±1.89%), whereas for the
grain size according to the percentage of clay (3.2±7.6%), silt (3.4±7.6%) and sand (93.3±15.1%) in the
sediments. The results of pH analysis show an increase of pH from 5.7 (acidic) to 8.5 (alkaline) as the
samplings are conducted from inland toward the sea. The lowest moisture content and organic matter
are 4.99% and 0.30% respectively, whereas the highest are 48.75% and 6.73% respectively. The textural
classification of coastal sediment are mostly sand. The percentage of clay and silt range from 0.05% to
25.3%, whereas the sand ranges from 49.4% to 99.7%.
Table 1. Average values for the physico-chemical properties of coastal sediments.
Station 1 2 3 4
Mean ±
Samples SP2 SP3 S1A S1B S2A S2B S2C S2D S3A S3B S4A S4B SM1 SM2 Range
SD
pH 5.7 6.5 7.1 7.9 7.3 7.8 7.9 7.5 7.3 7.7 8.4 8.5 6.1 6.4 5.7-8.5 7.29±0.98
MC % 5.0 5.8 25.0 25.8 24.0 23.8 15.3 25.3 26.2 39.9 25.9 27.9 35.4 48.8 4.9-48.8 25.3±12.9
OM % 0.3 0.3 0.3 0.3 0.2 0.2 0.2 0.1 0.3 0.8 1.6 1.8 4.7 6.7 0.1-6.7 1.27±1.89
Sand % 98.7 98.0 99.1 99.7 99.1 99.6 99.7 99.6 98.4 98.8 99.8 98.7 67.8 49.4 49.4-99.7 93.4±15.1
Silt % 0.55 1.07 0.46 0.20 0.05 0.30 0.25 0.25 1.02 0.91 0.10 0.91 16.1 25.3 0.05-25.3 3.4±7.6
Clay % 0.76 0.92 0.40 0.15 0.05 0.15 0.05 0.15 0.61 0.30 0.15 0.36 16.1 25.3 0.05-25.3 3.2±7.6
Texture S S S S S S S S S S S S SL SCL
S. sand, SL. sandy loam, SCL. sandy clay loam
3.2. Heavy Metal Content

Table 2 shows the total mean concentration of Fe (15,650±5,957 mg/kg), As (5.5±3.1 mg/kg), Cr
(78.3±37.2 mg/kg), Cu (15.7±10.4 mg/kg), Mn (298.1±127.4 mg/kg), Ni (159.0±75.0 mg/kg), Pb
(6.7±2.1 mg/kg) and Zn (29.5±11.9 mg/kg) in the fine grain <63μm fraction. The decreasing ranking
order for elemental concentrations is Fe>Mn>Ni>Cr>Zn>Cu>Pb>As. The heavy metal concentrations
are compared with the standard limits for coastal sediments based on the SQG established by US EPA
[32] as summarized in Table 2. The present study shows that all heavy metals are within the permissible
levels, except for Cr and Ni. When compared to the world’s average shale values (*ASV) as reference,
all heavy metals are below their respective background values, except for Cr and Ni which has exceed
4
the background values. The SQGs suggested that the current status for most of the heavy metals are non-
polluted except for Cr and Ni, implying these metals may pose threats to the marine environment.
Table 2. Total concentration of heavy metals in beach sediment and their background value.
Total Mean Concentration (mg/kg)

Station Sample
Fe As Cr Cu Mn Ni Pb Zn
SP2 17,232 3.7 89.9 13.1 324.7 183.6 6.8 40.5
1 SP3 15,775 2.1 78.6 10.5 228.3 168.3 5.9 43.7
S1A 17,399 9.7 95.5 9.9 375.0 185.5 2.5 43.5
S1B 21,040 12.2 117.9 11.4 540.9 225.3 4.3 43.4
S2A 15,638 4.1 86.4 10.8 259.4 178.2 8.2 36.1
S2B 18,612 7.8 135.6 10.8 375.7 208.2 9.1 40.3
2
S2C 16,274 7.5 123.7 9.7 370.8 189.6 6.2 39.2
S2D 18,115 6.7 112.0 10.8 317.8 197.0 8.1 40.6
S3A 19,785 3.4 96.1 15.2 245.6 200.6 7.6 51.4
3 S3B 21,196 4.8 79.0 18.7 319.8 168.4 7.3 51.3
S4A 4,476 3.4 9.0 31.4 137.2 11.7 2.5 19.4
4 S4B 5,373 3.2 8.2 40.7 102.7 9.1 4.3 22.1
Mean ± SD 15,650 ± 5,957 5.5 ± 3.1 78.3 ± 37.2 15.7 ± 10.4 298.1 ± 127.4 159 ± 75 6.7 ± 2.1 29.5 ± 11.9
*ASV 47,200 13 90 45 850 68 20 95
SQG by Non-Polluted <3 <25 <25 <300 <20 <40 <90

US EPA Moderate 3-8 25-75 25-50 300-500 20-50 40-60 90-200
High >8 >75 >50 >500 >50 >60 >200
3.3. Sediment Quality Assessment

Several pollution indices were determined for As, Cr, Cu, Mn, Ni, Pb and Zn including Igeo, EF, CF,
mCd and PLI to determine the extent of contamination by the heavy metals. From Table 3, all elements
show Igeo<0 indicating no pollution, except for Ni with 0≤Igeo<1, which corresponds to minor
contamination in the sediments. The EF values ranked as Ni>Cr>Cu>As>Zn>Mn>Pb which suggests
that Ni is the most enriched element in the study area. The mean EF show 1≤EF<3 for As (1.44), Cr
(2.62), Cu (1.66), Mn (1.09), Pb (0.99) and Zn (1.34), indicating minor enrichment by anthropogenic
inputs to the coastal sediments. Ni (6.37) shows 5≤EF<10, within Class 3 suggesting moderately severe
enrichment. Table 4 shows the mean CF values of heavy metals were ranked as
Ni>Cr>As>Zn>Cu>Mn>Pb, whereby all elements are CF<1 (low contamination), except Ni is 1≤CF<3
(moderate contamination). The mCd values for all stations are <1.5, suggesting nil to very low degree
of contamination in the study area, while the PLI revealed that the Kota Belud marine ecosystem has
low degree of contamination (0≤PLI<1). Station 4 which was located within the Crocker Formation
shows the lowest PLI values, compared to Station 1 to 3 which are made up of alluvial deposits and
largely influenced by the weathered mineral deposits from Wariu Formation.
5
Table 3. Igeo and EF parameters based on Turekian and Wedepohl (1961) as reference.
Geoaccumulation Index (Igeo) Enrichment Factor (EF)

Sample
As Cr Cu Mn Ni Pb Zn As Cr Cu Mn Ni Pb Zn
SP2 -2.38 -0.59 -2.37 -1.97 0.85 -2.14 -1.81 0.79 2.74 0.80 1.05 7.40 0.93 1.17
SP3 -3.19 -0.78 -2.69 -2.48 0.72 -2.34 -1.71 0.49 2.61 0.70 0.80 7.40 0.89 1.38
S1A -1.01 -0.50 -2.77 -1.77 0.86 -3.59 -1.71 2.02 2.88 0.60 1.20 7.40 0.34 1.24
S1B -0.68 -0.20 -2.56 -1.24 1.14 -2.79 -1.72 2.10 2.94 0.57 1.43 7.43 0.49 1.02
S2A -2.24 -0.64 -2.65 -2.30 0.81 -1.88 -1.98 0.96 2.90 0.72 0.92 7.91 1.23 1.15
S2B -1.32 0.01 -2.65 -1.76 1.03 -1.72 -1.82 1.52 3.82 0.61 1.12 7.77 1.16 1.08
S2C -1.39 -0.13 -2.79 -1.78 0.89 -2.28 -1.86 1.67 3.99 0.63 1.27 8.09 0.89 1.20
S2D -1.54 -0.27 -2.64 -2.00 0.95 -1.89 -1.81 1.34 3.24 0.63 0.97 7.55 1.05 1.11
S3A -2.51 -0.49 -2.15 -2.38 0.98 -1.97 -1.47 0.63 2.55 0.81 0.69 7.04 0.91 1.29
S3B -2.03 -0.77 -1.85 -2.00 0.72 -2.03 -1.47 0.82 1.95 1.56 0.84 5.51 0.82 1.20
S4A -2.54 -3.91 -1.10 -3.22 -3.12 -3.59 -2.88 2.72 1.05 4.39 1.70 1.82 1.31 2.15
S4B -2.59 -4.05 -0.73 -3.63 -3.48 -2.79 -2.69 2.19 0.80 7.94 1.06 1.18 1.91 2.04
Mean -1.95 -1.03 -2.25 -2.21 0.20 -2.42 -1.91 1.44 2.62 1.66 1.09 6.37 0.99 1.34
Table 4. CF, mCd and PLI parameters for the coastal sediment
Contamination Factor (CF) ΣCf mCd PLI

Samples
As Cr Cu Mn Ni Pb Zn
SP2 0.29 1.00 0.29 0.38 2.70 0.34 0.43 5.43 0.78 0.53
SP3 0.16 0.87 0.23 0.27 2.47 0.30 0.46 4.77 0.68 0.44
S1A 0.75 1.06 0.22 0.44 2.73 0.12 0.46 5.78 0.83 0.53
S1B 0.94 1.31 0.25 0.64 3.31 0.22 0.46 7.12 1.02 0.68
S2A 0.32 0.96 0.24 0.31 2.62 0.41 0.38 5.23 0.75 0.51
S2B 0.60 1.51 0.24 0.44 3.06 0.46 0.42 6.73 0.96 0.66
S2C 0.57 1.37 0.22 0.44 2.79 0.31 0.41 6.11 0.87 0.60
S2D 0.52 1.24 0.24 0.37 2.90 0.40 0.43 6.10 0.87 0.60
S3A 0.26 1.07 0.34 0.29 2.95 0.38 0.54 5.83 0.83 0.56
S3B 0.37 0.88 0.42 0.38 2.48 0.37 0.54 5.42 0.77 0.59
S4A 0.26 0.10 0.70 0.16 0.17 0.12 0.20 1.72 0.25 0.20
S4B 0.25 0.09 0.90 0.12 0.13 0.22 0.23 1.95 0.28 0.21
Mean CF 0.44 0.96 0.36 0.35 2.36 0.30 0.41
3.4. Pearson’s Correlation Matrix

Pearson’s correlation matrix defines the relationship between the contaminants in the sediment and their
potential common sources at significance level of p<0.01 (**strong correlation) and p<0.05 (*moderate
correlation). The correlation between the coefficients is displayed in Table 4, in which Fe is strongly
positive correlated with Cr (r=0.865**), Mn (r=0.783**), Ni (r=0.952**) and Zn (r=0.944**), but shows
no significance correlations with As, Cu and Pb. The As metal has a moderate positive correlation with
Cr (r=0.599*) and a strong positive correlation with Mn (r=0.863**). Cr also shows strong positive
correlation with Mn (r=0.830**), Ni (r=0.951**) and Zn (r=0.722**), whereas Ni is also strongly
positive correlated to Zn (r=0.855**). Pb is the only variable that shows no significance correlations to
all other coefficients. The other heavy metals also do not show any significant correlation with one other
when tested. A strong correlation between the heavy metals suggest that they originate from a common
natural or anthropogenic source, whereas a weak or no significant correlation indicate the metals are
from different pollution sources [33]. The Pearson correlation matrix of physico-chemical parameters
also show negative correlation between pH with heavy metals but show positive correlation between
organic matter and clay with heavy metals, all except for Cu metal.
6
Table 5. Pearson’s correlation matrix for the physico-chemical parameters and heavy metals.
pH OM Clay Fe As Cr Cu Mn Ni Pb Zn
pH 1
OM 0.701** 1
Clay -0.520 0.962** 1
Fe -0.657* 0.799** 0.831** 1
As -0.307 0.525 0.414 0.461 1
Cr -0.667** 0.894** 0.917** 0.865** 0.599* 1
Cu 0.472 -0.739** -0.815** -0.464 -0.383 -0.697* 1
Mn -0.399 0.709** 0.701** 0.783** 0.863** 0.830** -0.544 1
Ni -0.691** 0.916** 0.791** 0.952** 0.505 0.951** -0.681* 0.811** 1
Pb -0.581* 0.675** 0.520 0.531 -0.179 0.552 -0.187 0.139 0.537 1
Zn -0.635* 0.673** 0.733** 0.944** 0.253 0.722** -0.349 0.592* 0.855** 0.468 1
N=53, *Correlation is significant at the 0.05 level **Correlation is significant at the 0.01 level
4. Discussion
4.1. Physico-chemical Properties of Sediments

When metals are incorporated into sediments, they exist in the solid phase and are not readily available
for the marine ecosystem. However, changes in the physico-chemical conditions of sediments like pH
level, moisture, organic content and granulometric texture determine the bioavailability, mobility,
leachability and migration of heavy metals to other parts of the sediments which may impact the overall
sediment quality [34]. Other sediment characteristics such as the structure, bulk density, hydraulic
conductivity, permeability and porosity also influence the spatial distribution of the metal concentrations
in coastal areas [35,36]. The physico-chemical parameters also influence the biogeochemical processes
such as the oxidation and reduction of iron and manganese that facilitate the cycle of heavy metals from
sediments into the marine ecosystem and vice versa.
The pH levels are higher in the coastal region compared to the inland areas due to the intrusion
of highly alkaline and saline seawater from the South China Sea. Besides from the disintegration of
ultrabasic rock materials from Wariu Formation that accumulate along the beach shoreline, the
dissolution of bicarbonate materials from shelled organisms and corals also increases the alkaline
properties of coastal sediments [37,38]. The precipitation of certain heavy metals in the form of insoluble
oxides, hydroxides and carbonates may also contribute to the alkaline properties. In contrary, the higher
organic matter content in clastic sedimentary phases such as sandstone and shale increase the acidity of
inland sediments. Sediments with a higher clay percentage also have greater organic content due to the
higher binding ability of organic particles on the fine clay surfaces by adsorption-desorption kinetics,
which further contribute to the acidic conditions of the inland sediments [39,40].
The inconsistent moisture content fluctuates in a high variation from 4.9% to 48.8% due to the
difference in beach topography, capillary flow, complex storm-wave action, as well as the sea level
changes [17,41,42]. According to Schmutz and Namikas [43], the fluctuation of the moisture content
indicates the transitional zone (5-40%), where the moisture content decreases in the landward direction.
The cohesive-adhesive forces on the sand grains surface induced by surface moisture hold and resist the
uppermost layer of the sediments from being eroded into the ocean [16]. Surface moisture also limits
the entrainment of the beach sediment supply, thus preventing the heavy metal burden in sediments from
being easily released and remobilized back into the seawater column as secondary source of pollution
[44,45,46]. The carbonate materials released from dissolved shelled marine biota and corals provides a
stable archive for heavy metals in the form of insoluble and immobile carbonate-metal complexes,
whereby the heavy metals are retained and bioaccumulate in the sediments.
7
4.2. Possible Heavy Metal Sources

The spatial distribution of heavy metals in coastal sediments is controlled by natural and anthropogenic
factors such as the weathering of geological parent rocks, atmospheric conditions, oceanographic
environment, agriculture, transportation effluents, domestic waste and industrial wastewater [47,48,49].
Contaminants are transported via drainage system into the ocean basin, where the sediments serve as
natural sink for the accumulation of heavy metal burden. The mean enrichment factor suggested all
selected metals As, Cr, Cu, Mn, Pb and Zn originate from a mixture of both natural and anthropogenic
origins and their distributions are controlled by pH, moisture content, organic matter and grain size. Any
changes in the physico-chemical properties will lead to the release and resuspension of heavy metals
from sediments to the overlying marine water causing secondary pollution and deteriorates the marine
ecological system [50].
The high iron (Fe) and manganese (Mn) concentrations were derived from Fe-Mn oxide
fractions in clay particles from the oxidation and reduction processes during the pedogenesis of clastic
sedimentary rocks [56,57,58]. Fine clay minerals are principally associated with the silt-clay fraction
thus, they carry more Fe metal than coarse sand fraction as shown in Station 1 to 3, where alluvial
deposits have a higher clay content than in Crocker Formation. The high Fe2+/Fe3+ ratio in coastal
sediments is also due to the microbial reduction of Fe to form oxide minerals transported to the beach
shoreface where its mobility is restricted by the alkaline condition of the marine environment [59]. The
high Mn content is also contributed by carbonate materials of shelled organisms and assemblages of
calcareous benthic foraminifera in sediments [60,61,62]. The emission of hydrothermal vents on the
seafloor also creates an immense amount of Fe and Mn which will eventually precipitate and deposit
either on the seabed or circulated to the sediments along the beach shoreline [63,64,65]. This study
shows that the Fe and Mn act as complexing agent to form strong complexes with As, Cr, Ni and Zn.
Apart from atmospheric input, the oceanic hydrothermal nodules also produce particle plumes rich in
natural Zn, Pb, As and Cu emission in the marine chemistry [66]. The positive strong correlation
between Fe with Cr, Ni, Mn and Zn suggest that they originate from common geological source rocks,
either cherts and ultrabasic rocks (dismembered ophiolites) from Wariu formation, or from weathered
shale and sandstone from Crocker formation [61,67,68].
Nickel (Ni) has the highest mean CF and EF values, followed by chromium (Cr) which
suggested the metals are enriched by both lithogenic origins and human factors in the sediment. Organic
matter serves as a reductant for Cr element [51], therefore, the low OM and alkaline properties in coastal
regions allow Cr to remain stable and a fraction of Cr is retained in the sediments as insoluble
compounds along the beach shoreline [52]. Cr3+ tend to precipitate as insoluble Cr(OH)3 at higher pH
and bind to the sediment surface, thus increasing the affinity for Cr in alkaline soil and this may cause
detrimental impact on the sediment quality when the concentration level exceeds the acceptable limits.
From the present study, Cr and Ni shows a strong association as shown in Station 1 to 3 which
corresponds to the mineral deposits of weathered ultrabasic rocks from Wariu Formation in the coasts.
Ni is significantly higher than the other heavy metals due to the high mobility in surface sediments. The
strong association of Fe and Mn as potential carriers constitutes a significant sink for other heavy metals
in the sediments such as Cr, Ni, As and Pb as shown in Table 2. Stefania et al. [53] found that zinc (Zn)
concentrations decrease at higher pH due to a higher adsorption rate of Zn into the sediment which led
to metal retention and reduce in solubility, as can be seen in Station 4, whereby the Zn content is lower
under a higher pH condition in sediment. However, the water-soluble characteristic of Zn may
contaminate the marine ecosystem when the background values exceed and biomagnify in biota and the
bodies of marine organisms [54,55].
Other trace metals such as arsenic (As), copper (Cu) and lead (Pb) are released by human
interpolation such as agricultural, industrial and domestic activities, as they do not show any significant
correlation with other coefficients. The solubility and leachability of Cu is also influenced by the
sediment properties such as the organic matter content. Cu form strong complexes with the organic
matter in alkaline condition, which restrict the mobility of Cu, thereby only very small fraction of Cu is
available as ionic Cu2+ in sediments [69]. The present study also shows the relatively higher organic
8
matter in Station 4 serve as the complexing agent for Cu to bioaccumulate in the sediment. The strong
correlation between Cu and organic matter also suggested Cu is derived from the microbial degradation
of organic matter which releases soluble Cu into the marine environment. The concentration of As is the
lowest in the coastal region as the compounds are adsorbed strongly to the clastic sedimentary phases
from Crocker Formation and are transported only over short distances via groundwater or surface water
[9]. Although Pb concentration and EF is relatively low, the element corresponds to the anthropogenic
inputs by automotive exhaust emissions, untreated industrial effluents, domestic wastes and pesticide
spray. Since Pb shows only weak and insignificant correlation with other variables, this suggests that
Pb is released from different inputs. The domestic and industrial effluents from the inland regions are
commonly found precipitated of Pb as soluble oxide in which the metal is transported and leached to the
coastal regions [70].
4.3. Sediment Quality Assessment

The quality assessment of heavy metals is based on the statistical analysis and standard guidelines
applicable for heavy metals in coastal sediments. Sediment quality guidelines (SQGs) established by the
United States Environmental Protection Agency [32] are used to assess whether the heavy metals will
pose any threats to marine environment or lead to adverse biological impacts on the food chain that also
affect human health. When compared to the standard limits of SQGs, the overall mean concentrations
of Cu (15.7 mg/kg), Mn (298.1 mg/kg), Pb (6.7 mg/kg) and Zn (29.5 mg/kg) show no pollution nor large
variations, meanwhile As (5.5 mg/kg) is moderately polluted whereas Cr (78.3 mg/kg) and Ni (159
mg/kg) are highly polluted. Although their mean concentrations were lower than their respective ASVs,
except for Ni, the SQG suggests that these heavy metals serve as potential threats to the marine
ecosystem and long-term monitoring are required. Therefore, several pollution indices were conducted
to assess and interpret the current status of sediment quality in the Usukan coast.
Geoaccumulation index (Igeo) is used to compare the current contamination status of sediment
with that of the background concentration, as introduced by Müller [71]. The present study show there
is no serious accumulation of heavy metals along the beach shoreline and the sediments are practically
uncontaminated, except minor contamination by Ni. The effects of human interventions or heavy metal
enrichment in the coastal sediments were evaluated from the EF values [72,73]. Fe is chosen as the
reference element to create the regional geochemical baseline of heavy metals in this study and to
distinguish the heavy metals originating from either geological factors or human activities. The mean
EF values show that As, Cr, Cu, Mn, Pb and Zn are 1≤EF<3 which describe there are minor enrichment
of anthropogenic inputs in the sediments but 5≤EF<10 for Ni suggesting moderately severe enrichment.
This also means that all selected heavy metals for this study are of mixed origin from both lithogenic
(crust) origin, which is from the parent soil-forming rocks and anthropogenic sources [66]. Ni is
significantly higher due to its high mobility to be transported over a large distance from source rocks
into the coastal areas, with the aid of Fe-Mn metal complexes as carriers.
Contamination factor (CF) is commonly used to assess the extent of sediment contamination in
coastal environment due to toxicity of heavy metals. From the present study, all metals show CF<1
indicating low contamination level, except for Ni that show moderate contamination level (1<CF<3).
The sum of the contamination factor (ΣCF) was also calculated using the modified contamination degree
equation (mCd) introduced by Hakanson [74]. However, the mCd values for each station sum up the
factor analysis to <1.5 which suggests very low degree of contamination by anthropogenic sources in
the Kota Belud marine ecosystem. Pollution load index (PLI) was also derived from the mean values of
contamination factors (CF) for every metal present in the study area to that of natural background value,
as proposed by Tomlinson et al. [75]. The PLI revealed all sampling stations has only low degree of
pollution (0≤PLI<1), indicating very low deterioration of the sediment quality. The overall values of
both mCd and PLI correspond to the minor effect of anthropogenic sources on the current status of heavy
metal pollution in the coastal sediments.
9
5. Conclusion
The heavy metals assessment revealed only minimal degree of pollution in the coastal sediments.
Geochemical analysis shows a decreasing ranking order of the elemental concentration
Fe>Mn>Ni>Cr>Zn>Cu>Pb>As, whereby Fe is selected as the reference element for the study of
sediment quality assessment. The analyses show all elements are lower than their respective world’s
average shale values and within the acceptable standard limits of the Sediment Quality Guidelines by
US EPA for coastal sediments, except Ni. The physico-chemical parameters conducted for the coastal
sediments are the pH conditions (range 5.6-8.5), moisture content (mean 25.3%), organic matter (mean
1.27%) and grain size (mean sand 93.4%, silt 3.4%, clay 3.2%) that affect the mobility, leaching,
distribution and accumulation of the heavy metals in sediments. Pearson’s correlation analysis shows
that the heavy metal content is mainly from the geological source rocks, either sedimentary rocks from
Crocker Formation or dismembered ophiolites from Wariu Formations which are transported from
inland to the coastal regions of Usukan beach. The mCd and PLI values suggest that Kota Belud marine
ecosystem is only affected by low degree of contamination by anthropogenic sources and the current
status of the study area is safe from pollution. However, a long-term monitoring of the marine
environment is required to assess the contamination level and quality status of the coastal sediments.
Acknowledgement
We are grateful to Universiti Malaysia Sabah for providing the laboratory facilities at Faculty of Science
and Natural Resources and Ministry of Higher Education of Malaysia for the financial support with
Project Code TR@M001-2019.
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Geochemical Assessment of Heavy Metal Contamination in Coastal Sediment Cores From Usukan Beach, Kota Belud, Sabah, Malaysia

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GEOCHEMICAL ASSESSMENT OF HEAVY METAL

Keywords: Geochemistry, Heavy Metal, Contamination, Sediment Quality, Coast

2. Materials and Methodology

2.1. Sampling Location and Technique

2.2. Laboratory Analysis

2.3. Statistical Analysis

3.1. Physico-chemical Properties

Table 1. Average values for the physico-chemical properties of coastal sediments.

S. sand, SL. sandy loam, SCL. sandy clay loam

3.2. Heavy Metal Content

Total Mean Concentration (mg/kg)

SQG by Non-Polluted <3 <25 <25 <300 <20 <40 <90

3.3. Sediment Quality Assessment

Geoaccumulation Index (Igeo) Enrichment Factor (EF)

Contamination Factor (CF) ΣCf mCd PLI

3.4. Pearson’s Correlation Matrix

4.1. Physico-chemical Properties of Sediments

4.2. Possible Heavy Metal Sources

4.3. Sediment Quality Assessment

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